Optimizing Ion Transport in Polyether-Based Electrolytes for Lithium Batteries

Zheng, Qi; Pesko, Danielle M.; Savoie, Brett M.; Timachova, Ksenia; Hasan, Alexandra L.; Smith, Mackensie C.; Miller, Thomas F.; Coates, Geoffrey W.; Balsara, Nitash P.

doi:10.1021/acs.macromol.7b02706

Optimizing Ion Transport in Polyether-Based Electrolytes for Lithium Batteries

Journal Article · Tue Apr 03 00:00:00 EDT 2018 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.7b02706· OSTI ID:1461983

Zheng, Qi ^[1]; ^[2]; Savoie, Brett M. ^[3]; ^[2]; Hasan, Alexandra L. ^[4]; Smith, Mackensie C. ^[2]; ^[5]; ^[1]; ^[6]

Cornell Univ., Ithaca, NY (United States). Dept. of Chemistry and Chemical Biology. Baker Lab.
Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
Purdue Univ., West Lafayette, IN (United States). Charles D. Davidson School of Chemical Engineering
Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering
Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division. Energy Storage and Distributed Resources Division

In this paper, we report on the synthesis of poly(diethylene oxide-alt-oxymethylene), P(2EO-MO), via cationic ring-opening polymerization of the cyclic ether monomer, 1,3,6-trioxocane. We use a combined experimental and computational approach to study ion transport in electrolytes comprising mixtures of P(2EO-MO) and lithium bis(trifluoromethanesulfonyl) imide (LiTFSI) salt. Mixtures of poly(ethylene oxide) (PEO) and LiTFSI are used as a baseline. The maximum ionic conductivities, σ, of P(2EO-MO) and PEO electrolytes at 90 °C are 1.1 × 10^–3 and 1.5 × 10^–3 S/cm, respectively. This difference is attributed to the T_g of P(2EO-MO)/LiTFSI (-12 °C), which is significantly higher than that of PEO/LiTFSI (-44 °C) at the same salt concentration. Self-diffusion coefficients measured using pulsed-field gradient NMR (PFG-NMR) show that both Li⁺ and TFSI^– ions diffuse more rapidly in PEO than in P(2EO-MO). However, the NMR-based cation transference number in P(2EO-MO) (0.36) is approximately twice that in PEO (0.19). The transference number measured by the steady-state current technique, t_+,ss, in P(2EO-MO) (0.20) is higher than in PEO (0.08) by a similar factor. We find that the product σt_+,ss is greater in P(2-EO-MO) electrolytes; thus, P(2EO-MO) is expected to sustain higher steady-state currents under dc polarization, making it a more efficacious electrolyte for battery applications. Molecular-level insight into the factors that govern ion transport in our electrolytes was obtained using MD simulations. These simulations show that the solvation structures around Li⁺ are similar in both polymers. The same is true for TFSI^–. However, the density of Li⁺ solvation sites in P(2EO-MO) is double that in PEO. Finally, we posit that this is responsible for the observed differences in the experimentally determined transport properties of P(2EO-MO) and PEO electrolytes.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF) (United States); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1461983

Journal Information:: Macromolecules, Journal Name: Macromolecules Journal Issue: 8 Vol. 51; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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